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Elastic and inelastic helium atom scattering experiments have been carried out on the KTaO 3 (001) surface, prepared by cleaving in situ under ultra high vacuum conditions. Several unusual observations were recorded in the helium diffraction studies. These include the appearance of metastable surface features immediately after cleaving ͑which decay to the stable (1ϫ1) surface after a few hours͒, the formation and dissolution of small (2ϫ1) and (1ϫ2) domains depending on the thermal history of the surface, large hysteresis in the diffraction beam intensities measured for surface temperatures between 200 K and 50 K depending on whether the surface is being warmed or cooled, and permanent changes in the diffraction intensities as a result of poling normal to the surface plane. The single-phonon energy-transfer experiments yield three surface phonon dispersion branches in the ͗100͘ and ͗110͘ high-symmetry azimuths. Calculations of the lattice dynamics using the VASP approach are described and the results are compared with the measurements.

The surface structure and vibrations of normal-H 2 , para-H 2 , HD, and normal-D 2 films physisorbed on in situ cleaved single crystal MgO͑001͒ surfaces, have been investigated at surface temperatures 7-12 K using high-resolution helium atom scattering. The He-diffraction patterns agree with the sequence of c(2ϫ2)c(4ϫ2)-c(6ϫ2) structures previously determined by neutron scattering. For the H 2 monolayer three different adsorbate frequencies, two Einstein modes around 10 meV and a dispersive mode between 2 and 7 meV, are found. HD and D 2 show the expected isotopomer shifts. A second probably ordered H 2 layer is formed upon further adsorption and exhibits one dispersionless mode at 5 meV.

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